Epitaxial synthesis of ultrathin β-In2Se3/MoS2 heterostructures with high visible/near-infrared photoresponse

van der Waals (vdWs) heterostructures, combining different two-dimensional (2D) layered materials with diverse properties, have been demonstrated to be a very promising platform to explore a new physical phenomenon and realize various potential applications in atomically thin electronic and optoelectronic devices. Here, we report the controlled growth of vertically stacked β-In2Se3/MoS2 vdWs heterostructures (despite the existence of large lattice mismatching ∼29%) through a typical two-step chemical vapor deposition (CVD) method. The crystal structure of the achieved heterostructures is characterized by transmission electron microscopy, where evident Moiré patterns are observed, indicating well-aligned lattice orientation. Strong photoluminescence quenching is obeserved in the heterostructure, revealing effective interlayer charge transfer at the interface. Electrical devices are further constructed based on the achieved heterostructures, which have a high on/off ratio and a typical rectifying behavior. Upon laser irradiation, the devices show excellent photosensing properties. A high responsivity of 4.47 A W-1 and a detectivity of 1.07 × 109 Jones are obtained under 450 nm laser illumination with a bias voltage of 1 V, which are much better than those of heterostructures grown via CVD. Most significantly, the detection range can be extended to near-infrared due to the relatively small bandgap nature of β-In2Se3. With 830 nm laser illumination, the devices also show distinct photoresponses with fast response speed even when operating at room temperature. The high-quality β-In2Se3/MoS2 heterostructures broaden the family of the 2D layered heterostructure system and should have significant potential applications in high-performance broadband photodetectors.